COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Zhongjian Wang,Guojun Lv,Jingbo Wang,Zhuoran Zhang,Yuhan Jiang,Yangbin Shen
The strong d-p covalent interaction of Mo-P bonds was obtained. • Lattice doping of P into MoS 2 formed Mo-P bonds in 0.2P-MoS 2. • 0.2P-MoS 2 achieved 91.7% tetracycline degradation under LED irradiation. Antibiotic pollution in water calls for sustainable remediation approaches such as photocatalysis. Despite its promising structure and visible-light response, MoS 2 is hindered by rapid carrier recombination, which severely restrict its photocatalytic efficiency. Herein, we reported a strategy of lattice phosphorus doping into MoS 2 to modulate the electronic structure, broaden visible-light absorption, and facilitate charge separation and migration. The optimized 0.2P-MoS 2 achieved 91.7% degradation of tetracycline (30 mg/L) within 80 min under low-power LED irradiation, with a reaction rate constant 5.5-fold higher than pristine MoS 2 . The superior photocatalytic degradation activity for 0.2P-MoS 2 arises from the narrowest band gap (1.21 eV) and accelerated charge carrier migration originated from the strong d-p covalent interactions in the generated Mo-P bonds. Radical scavenging experiments and electron paramagnetic resonance characterizations identified superoxide radicals (•O 2 − ) and holes (h⁺) as the dominant reactive species. Furthermore, possible photocatalytic degradation pathways of tetracycline were proposed over the 0.2P-MoS 2 catalyst. Moreover, the 0.2P-MoS 2 catalyst maintained high activity after five consecutive cycles, demonstrating its excellent stability. This work offers an electronic structure engineering perspective for rational design of MoS 2 -based photocatalysts and provides a viable approach for antibiotic degradation under low-power light sources, holding substantial promise for environmental remediation. Download: Download high-res image (187KB) Download: Download full-size image Strong d-p orbital hybridization of Mo-P bonds within phosphorus lattice-doped MoS 2 boosts visible-light photocatalytic degradation of tetracycline into CO 2 and H 2 O.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Gaili Ke,Feng Duan,Binyao Liu,Xiaotian Liu,Jinyu Wen,Bi Jia,Xiaoyan Liu,Huichao He,Yong Zhou
In theory, suitable metal ions doping into the surface of BiVO 4 photoanodes could improve its water oxidation performance effectively. But the common homogeneous reaction strategy is not well applicable for the preparation of BiVO 4 film photoanodes with metal ions surface doping. Herein, a photoelectrochemical treating approach was reported to prepare BiVO 4 films with W or Mo surface doping in saturated tungstate and molybdate-containing electrolyte, respectively. The doping of W or Mo into the surface of BiVO 4 film was attributed to the following reactions. Firstly, the photocorrosion of BiVO 4 film photoelectrodes resulted in the dissolution of VO 4 3+ from BiVO 4 lattice under AM 1.5 G illumination. Then, the WO 4 2+ or MoO 4 2+ in the saturated electrolyte entered and occupied the dissolved sites of VO 4 3+ on BiVO 4 surface through ions exchange reaction . Due to the lower radiative recombination of carrier as well as higher electrocatalytic water oxidation activity, the resultant W or Mo doped BiVO 4 films as photoanodes showed better solar water oxidation activity, kinetics and stability, although their light harvesting property and morphological feature were close to the pristine BiVO 4 film photoanode. The present work provides a new and effective approach for the achievement of metal ions doping into the surface of BiVO 4 photoanodes, which could inspire the preparation of similar photoanode materials.
研究领域:
材料科学
·
能源科学
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Small Methods
·
2023
·Vol. 7
·期 8
·2300054
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IF 12.4
Lu Chen,Youbing Li,Kun Liang,Ke Chen,Mian Li,Shiyu Du,Zhifang Chai,Michael Naguib,Qing Huang
Two-dimensional (2D) transition metal carbides and/or nitrides, MXenes, are prepared by selective etching of the A-site atomically thin metal layers from their MAX phase precursors. High entropy MXenes, the most recent subfamily of MXenes, are in their infancy and have attracted great interest recently. They are currently synthesized mainly through wet chemical etching of Al-containing MAX phases, while various MAX phases with A-sites elements other than Al have not been explored. It is important to embody non-Al MAX phases as precursors for the high entropy MXenes synthesis to allow for new compositions. In this work, it is reported on the design and synthesis of Ga-containing medium/high entropy MAX phases and then their corresponding medium/high entropy MXenes. Gallium atomic layer etching is carried out using a Lewis acid molten salt (CuCl2). The as-prepared (Ti 1/4 V 1/4 Nb 1/4 Ta 1/4 ) 2 CT x exhibits a Li + specific capacity of ≈400 mAh g −1 . For (Ti 1/5 V 1/5 Nb 1/5 Ta 1/5 Mo 1/5 ) 2 CT x a specific capacity of 302 mAh g −1 is achieved after 300 cycles, and high cycling stability is observed at high current densities. This work is of great significance for expanding the family members of MXenes with tunable chemistries and structures.
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DOI
PubMed
高影响因子
Nanoscale
·
2022
·Vol. 15
·期 1
·259-265
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IF 8.307
Lin Tian,Zhenyang Chen,Tingjian Wang,Ming Cao,Xinhua Lu,Wenjing Cheng,Changchun He,Ju Wang,Zhao Li
Oxygen evolution reactions (OERs) are regarded as the rate-determining step of electrocatalytic overall water splitting, which endow OER electrocatalysts with the advantages of high activity, low cost, good conductivity, and excellent stability. Herein, a facile H2O2-assisted etching method is proposed for the fabrication of Mo-doped ultrathin Co9Se8@NiSe/NF-X heterojunctions with rich Se vacancies to boost electrocatalytic water oxidation. After step-by-step electronic structure modulation by Mo doping and Se vacancy engineering, the self-standing Mo-Co9Se8@NiSe/NF-60 heterojunctions deliver a current density of 50 mA cm−2 with an overpotential of 343 mV and a cell voltage of only 1.87 V at 50 mA cm−2 for overall water splitting in 1.0 M KOH. Our study opens up the possibility of realizing step-by-step electronic structure modulation of nonprecious OER electrocatalysts via heteroatom doping and vacancy engineering.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiahe Li,Weihong Wu,Rui Duan,Xue Bi,Weihua Meng,Jianzhong Xu,Hongqiang Qu
A molybdenum-based metal organic framework (Mo-MOF) and graphene oxide (GO) hybrid functionalized with boron-containing ionic liquid ([BMIM]BF 4 ) (GMB) was reported to effectively improve the fire safety and mechanical property of epoxy resin (EP). When 3 wt% GMB was added, the CO production rate, peak heat release rate and peak smoke release rate of EP composites decreased by 55.88%, 52.10% and 40.12%, respectively. The flame retardant mechanism was the combination of catalytic carbonization ([BMIM]BF 4 and Mo-MOF), physical barrier effect (GO) and gas phase dilution (H 2 O and NH 3 in gas production). Meanwhile, the incorporation of [BMIM]BF 4 endowed EP composites with excellent mechanical properties.
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Molecular Catalysis
·
2022
·
IF 5.089
Zhengting Xiao,Qingyang Li,Wentai Wang,Guangci Li,Guannan Lin,Xuebing Li,Song Chen
A Co-Mo sulfide catalyst with tube-like structure was prepared through a low-temperature pre-sulfurization process using rod-like CoMoO 4 as the precursor. The pre-sulfurization temperature greatly affected the total pore volume, the concentration of CoMoS species, the microstructure of (Co)MoS 2 slabs and the catalytic desulfurization activity. The increased temperature can promote the formation of hollow structure and the sulfurization degree of the precursor. It was found that the excessive temperature induced the Co atoms to form more isolated Co 9 S 8 species, hindering the formation of highly active CoMoS species. Therefore, appropriate temperature is more favorable to form the (Co)MoS 2 slabs with shorter length and higher stacking number, leading to more coordinatively unsaturated sites, especially the corner sites. According to the results of hydrodesulfurization reaction, the reaction rate of dibenzothiophene and the yields of liquid products are highly depended on the number of surface-active sites, which are mainly originated from the Type II CoMoS species. Moreover, the extended pre-sulfurization time can further improve the catalytic desulfurization activity of the catalyst at an appropriate pre-sulfurization temperature.
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高影响因子
FUEL
·
2022
·
IF 8.035
Minghao Zhou,Yaqi Xue,Fei Ge,Jing Li,Haihong Xia,Junming Xu,Jun Zhao,Changzhou Chen,Jianchun Jiang
MOF-derived Ni-based bimetallic catalysts were found to be effective for the in-situ hydrogenation/hydrodeoxygenation of lignin-derived monophenols and dimers with isopropanol as the hydrogen-donor solvent (without external hydrogen). The synergistic effects of bimetallic catalysts were studied, and their catalytic properties afforded the best conversion rate of phenols and cyclohexanol/cycloalkane yields. The detailed physicochemical characterization was conducted by means of XRD, H 2 -TPR, NH 3 -TPD, and pyridine-IR analysis. The effects of reaction temperature (200–260 ℃) and reaction time (2–5 h) on the performance of lignin-derived monophenols and dimers were investigated. During the in-situ hydrogenation/hydrodeoxygenation of lignin-derived phenols, the steric effects and the effects of various functional groups, notably methoxy groups, were investigated. In-situ conversion of lignin-derived phenols with isopropanol was achieved over different Ni/M ratios of NiM@C (M = Co, Mo, and La) catalysts, from which NiLa 0.33 @C produced satisfactory yields of cyclohexanol/cycloalkanes.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 20
·9887-9893
·
IF 3.3
Yao Tang,Zijun Zou,Xingen Wu,Pengfei Zuo,Lei Wang,Guiwen Huang,Jia Zhu,Shengliang Zhong
Designing highly efficient non-precious metal electrocatalysts to facilitate overall water decomposition is critical and highly desirable, but still challenging. In this study, we synthesized ZIF-67@POM nanomaterials by doping H3PMo12O40 in ZIF-67. The molybdenum-doped carbon matrix can effectively reduce CoP agglomeration, which is conducive to improving the specific surface area and active sites of the catalyst. The doping of Mo also optimizes the electronic structure of Mo-CoP-100 and improves its electrocatalytic activity. Compared with CoP derived from pristine ZIF-67, the optimal Mo-CoP-100 exhibits significantly enhanced oxygen evolution reaction (OER) catalytic activity with an almost constant overpotential of 290 mV to maintain a stable current density of 10 mA cm−2 in alkaline media for at least 100 h. Furthermore, compared with traditional precious metal-free OER electrocatalysts, the Mo-CoP catalysts prepared in this work have high specific surface area, rich surface-active sites, good cycling stability and high diffusion efficiency.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Caijuan Zhong,Shengxiao Zhang,Shuangshuang Yang,Baiqing Yuan,Qiang Xu,Zengrun Xie,Chenyu Du
Mo and N co-doped iron biochar material (Fe/Mo x -NC) was prepared through one-pot calcination method with anhydrous iron chloride, ammonium molybdate, and cherry stone powder as precursors. The composite can effectively catalyze activation of peroxymonosulfate (PMS) for organic pollutants degradation, and the removal rate of 20 mg/L bisphenol A (BPA) reaches 99.08% in 30 min in the presence of 0.1 g/L Fe/Mo 0.1 -NC and 1 g/L PMS. Electrochemical analysis indicates that appropriate doped Mo and N can improve the electron transfer performance of the composite, which enhances the PMS activation property for BPA degradation. Quenching experiments and electron paramagnetic resonance analysis both demonstrated that the Fe/Mo 0.1 -NC/PMS system generated SO 4 •− , •OH and 1 O 2 , which involved in BPA degradation. Moreover, a galvanic oxidation process had shown that there existed nonradical pathway which relied on electron transfer. The degradation pathway is proposed by measuring the intermediate products with HPLC-HRMS/MS. Through the exploration of the reaction mechanism, low-valence molybdenum ions can promote the cycle of Fe 2+ /Fe 3+ , and the pyridine-N and graphitic-N contained in Fe/Mo 0.1 -NC can catalyze activation of PMS together with Fe 2+ . The designed membrane filtration device revealed the feasibility of the composite in dynamic process, which was great significant for actual operation of water treatment. Furthermore, the Fe/Mo 0.1 -NC/PMS system could effectively decompose organic pollutants in the effluent from sewage treatment plant, achieving 82.6% of total organic carbon removal rate. This study not only prepared a novel heteroatom doped Fe-biochar material for PMS activation to degrade organic pollutants, but also deepened the reaction mechanism and explored its applicability for advanced treatment of real wastewater.
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Journal of Water Process Engineering
·
2023
·
IF 7
Caifeng Wei,Yanqin Cai,Zujin Yang
The presence of heavy metal ions and organic dyes in aqueous solutions has a significant impact on the ecological environment and human health. Herein, a novel bifunctional imidazolium-based porous organic polymer (IMSPF-Br-C=C) was prepared successfully via quaternization reaction of spirobifluorene and 1,4-dibromo-2-butene. The synthesized material was characterized by scanning electron microscopy (SEM) with energy dispersive spectroscopy (EDS), Fourier transform infra-red spectra (FTIR), Thermogravimetric analysis (TGA), X-ray diffraction (XRD), N 2 adsorption-desorption analysis and solid-state 13 C CP/MAS NMR spectroscopy, confirming its structure and stability. Owing to the conjugated structure of spirobifluorene, IMSPF-Br-C=C showed excellent recognition performance for dichromate anion (Cr 2 O 7 2− ) with the limit of detection (LOD) of 1.58 μmol/L. In addition, IMSPF-Br-C=C with the abundant imidazolium cations showed the outstanding adsorption performance in the removal of Cr 2 O 7 2− and methyl orange (MO). Removal efficiencies and adsorption capacities of IMSPF-Br-C=C were 98.3 % and 99.4 %, 452.8 and 1304.2 mg/g in 6 min, respectively. The results show that the electrostatic interactions and π-π stacking play crucial roles in the fluorescence detection of Cr 2 O 7 2− and adsorptive separation of Cr 2 O 7 2− and MO. Furthermore, physico-chemical techniques, density functional theory (DFT) calculation and frontier molecular orbital theory (FMO) were used to explain action mechanism. This work provides a cost-effective IMSPF-Br-C=C as a bifunctional platform for sensing Cr 2 O 7 2− and adsorptive separation of Cr 2 O 7 2− and MO in aqueous solution.
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高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 43
·23270-23277
·
IF 11.9
Xiaoyun Zhang,Shifan Zhu,Yixue Xu,Yuqiao Wang
The tip effect of the high curvature tip top can cause electromagnetic effects to improve the catalytic performance. Doping of transition metals (Cr, Fe and Mo) into CoP array nanocones alters the tip curvature of CoP to strengthen the tip effect with increasing curvature. The stronger tip effect of Fe-CoP improves OH− concentration, accelerates surface charge transfer and enhances the electric field for a higher catalytic efficiency. Fast charge transfer and high electronic conductivity are attributed to transition metal doping, which can be confirmed by theoretical simulations and experiments. The optimized d-band centre of Fe-CoP adjusts the appropriate adsorption strength of the reaction intermediates. Fe doping endows CoP with a higher curvature cone structure and optimizes electronic structure for high catalytic activity and reaction kinetics. Tip cone as special sites tuned by transition metal doping provides a strategy for efficient non-noble metal catalysis.
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2021
·
IF 8.067
Sainan Liu,Hongtai Shen,Jiawei Xu,Xiaojun Zhou,Jianfei Liu,Zhenyang Cai,Xiaojun Zhao,Lairong Xiao
To develop an ultra-high-temperature resistant coating for a reusable thermal protection system, the preparation of a tantalum-based MoSi 2 -Mo coating by a new two-step process of multi-arc ion plating and halide activated pack cementation is presented. The coating has a dense structure and is well compatible with the tantalum substrate, which can be thermally shocked from room temperature to 1750 °C for 360 cycles without failure. The mechanism of the coating’s excellent resistance to high-temperature thermal shocks is that a strong-binding gradient interface and a dense SiO 2 oxide scale with good oxygen resistance are formed by the high-temperature self-diffusion of Si.
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